Uric acid(UA)detection is essential in diagnosis of arthritis,preeclampsia,renal disorder,and cardiovascular diseases,but it is very challenging to realize the required wide detection range and low detection limit.We ...Uric acid(UA)detection is essential in diagnosis of arthritis,preeclampsia,renal disorder,and cardiovascular diseases,but it is very challenging to realize the required wide detection range and low detection limit.We present here a single-atom catalyst consisting of Co(Ⅱ)atoms coordinated by an average of 3.4 N atoms on an N-doped graphene matrix(A-Co-NG)to build an electrochemical biomimetic sensor for UA detection.The A-Co-NG sensor achieves a wide detection range over 0.4-41,950μM and an extremely low detection limit of 33.3±0.024 nM,which are much better than previously reported sensors based on various nanostructured materials.Besides,the A-Co-NG sensor also demonstrates its accurate serum diagnosis for UA for its practical application.Combination of experimental and theoretical calculation discovers that the catalytic process of the A-Co-NG toward UA starts from the oxidation of Co species to form a Co^3+-OH-UA*,followed by the generation of Co^3+-OH+^*UA_H,eventually leading to N-H bond dissociation for the formation of oxidized UA molecule and reduction of oxidized Co^3+to Co^2+for the regenerated A-Co-NG.This work provides a promising material to realize UA detection with wide detection range and low detection limit to meet the practical diagnosis requirements,and the proposed sensing mechanism sheds light on fundamental insights for guiding exploration of other biosensing processes.展开更多
基金the National Natural Science Foundation of China(Nos.22075195,21705115,21972102,and 21775122)the Natural Science Foundation of Jiangsu Province of China(BK20170378)+1 种基金Jiangsu Specially Appointed Professor program,the Natural Science research Foundation of Jiangsu Higher Education Institutions(17KJB150036)the Jiangsu Laboratory for Biochemical Sensing and Biochip.Natural Science Foundation of Chongqing(cstc2018jcyjAX0693),China.
文摘Uric acid(UA)detection is essential in diagnosis of arthritis,preeclampsia,renal disorder,and cardiovascular diseases,but it is very challenging to realize the required wide detection range and low detection limit.We present here a single-atom catalyst consisting of Co(Ⅱ)atoms coordinated by an average of 3.4 N atoms on an N-doped graphene matrix(A-Co-NG)to build an electrochemical biomimetic sensor for UA detection.The A-Co-NG sensor achieves a wide detection range over 0.4-41,950μM and an extremely low detection limit of 33.3±0.024 nM,which are much better than previously reported sensors based on various nanostructured materials.Besides,the A-Co-NG sensor also demonstrates its accurate serum diagnosis for UA for its practical application.Combination of experimental and theoretical calculation discovers that the catalytic process of the A-Co-NG toward UA starts from the oxidation of Co species to form a Co^3+-OH-UA*,followed by the generation of Co^3+-OH+^*UA_H,eventually leading to N-H bond dissociation for the formation of oxidized UA molecule and reduction of oxidized Co^3+to Co^2+for the regenerated A-Co-NG.This work provides a promising material to realize UA detection with wide detection range and low detection limit to meet the practical diagnosis requirements,and the proposed sensing mechanism sheds light on fundamental insights for guiding exploration of other biosensing processes.
